Fe<sub>3</sub>O<sub>4</sub>-nZVI类Fenton法降解水中磺胺甲恶唑

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Abstract Fe₃O₄-nZVI was prepared by co-precipitation and liquid phase reduction method. The obtained Fe₃O₄-nZVI was used as catalyst of Fenton-like reaction to degrade sulfamethoxazole (SMX) in water. The effects of H₂O₂ concentration, Fe₃O₄-nZVI dosage, pH of solution, SMX concentration and temperature on SMX degradation were investigated. The charactering results of SEM, EDS, XRD and XPS showed that the magnetic composite material with nanometer size was successfully prepared. The batch experimental results showed that the degradation rate of SMX in Fenton-like system increased as the increase of H₂O₂ concentration, Fe₃O₄-nZVI dosage and temperature, and decrease of pH in studied experimental ranges. The fitting parameters of kinetic showed that SMX degradation fitted the pseudo-first-order kinetic model. Under the given conditions, which were H₂O₂ 10mmol/L, Fe₃O₄-nZVI 0.8g/L, pH=3, SMX 10mg/L, and reaction temperature 25℃, the degradation rate of SMX was 99.61% at 180min. The magnetization of Fe₃O₄-nZVI was 105.52emu/g, indicating it was easy for magnetic recycle. Reused experiments showed that Fe₃O₄-nZVI had excellent reactivity and stability. Free radical quenching experiments showed that the oxidation of ·OH played a key role on degrading SMX in water.

Key words： Fe₃O₄-nZVI advanced oxidation Fenton-like sulfamethoxazole

Received: 09 December 2021

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X703.1

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	XIE Xin-zhuo
	ZHONG Jin-kui
	LI Jing
	ZHENG Bo-Wen

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XIE Xin-zhuo,ZHONG Jin-kui,LI Jing等. Degradation of sulfamethoxazole in water by Fenton-like method using Fe₃O₄-nZVI[J]. CHINA ENVIRONMENTAL SCIENCECE, 2022, 42(7): 3103-3111.

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http://www.zghjkx.com.cn/EN/ OR http://www.zghjkx.com.cn/EN/Y2022/V42/I7/3103

[1]	Dmitrienko S G, Kochuk E V, Apyari V V, et al. Recent advances in sample preparation techniques and methods of sulfonamides detection-A review[J]. Analytica Chimica Acta, 2014,850:6-25.
[2]	赵富强,高会,张克玉,等.中国典型河流水域抗生素的赋存状况及风险评估研究[J].环境污染与防治, 2021,43(1):94-102. Zhao F Q, Gao H, Zhang K Y, et al. Occurrence and risk assessment of antibiotics in typical river basins in China[J]. Environmental Pollution&Control, 2021,43(1):94-102.
[3]	张晶晶,陈娟,王沛芳,等.中国典型湖泊四大类抗生素污染特征[J].中国环境科学, 2021,41(9):4271-4283. Zhang J J, Chen J, Wang P F, et al. Pollution characteristics of four-type antibiotics in typical lakes in China[J]. China Environmental Science, 2021,41(9):4271-4283.
[4]	Yang B, Tian Z, Zhang L, et al. Enhanced heterogeneous Fenton degradation of Methylene Blue by nanoscale zero valent iron (nZVI) assembled on magnetic Fe3O4/reduced graphene oxide[J]. Journal of Water Process Engineering, 2015,5:101-111.
[5]	陈勇,胡鹭,谭旎,等.Al0-Gr-Fe0活化O2类Fenton氧化降解土霉素的研究[J].中国环境科学, 2021,41(10):4645-4653. Chen Y, Hu L, Tan N, et al. Oxidative degradation of oxytetracycline by a Fenton-like process with Al0-Gr-Fe0activated of O2[J]. China Environmental Science, 2021,41(10):4645-4653.
[6]	Lv D, Zhou X, Zhou J, et al. Design and characterization of sulfide-modified nanoscale zero valent iron for cadmium (II) removal from aqueous solutions[J]. Applied Surface Science, 2018,442:114-123.
[7]	Zou Y, Wang X, Khan A, et al. Environmental remediation and application of nanoscale zero-valent iron and its composites for the removal of heavy metal ions:a review[J]. Environmental Science&Technology, 2016,50(14):7290-7304.
[8]	Wu Y, Zhang J, Tong Y, et al. Chromium (VI) reduction in aqueous solutions by Fe3O4-stabilized Fe0 nanoparticles[J]. Journal of Hazardous Materials, 2009,172(2/3):1640-1645.
[9]	徐海玉,张明青,陈翌昱.有机凹凸棒石负载纳米零价铁去除水中六价铬[J].中国环境科学, 2019,39(12):5079-5084. Xu H Y, Zhang M Q, Chen Y Y. Removal of Cr (VI) from aqueous solution using organically modified attapulgite-supported nanoscale zero-valent iron[J]. China Environmental Science, 2019,39(12):5079-5084.
[10]	Lyu H, Tang J, Huang Y, et al. Removal of hexavalent chromium from aqueous solutions by a novel biochar supported nanoscale iron sulfide composite[J]. Chemical Engineering Journal, 2017,322:516-524.
[11]	邓俊敏.生物炭负载纳米零价铁在还原及氧化体系下对污染物的去除研究[D].长沙:湖南大学, 2018. Deng J M. A study on the application of nanoscale zero-valent iron/biochar composite on remediation of contaminated water in both reducing and oxidizing system[D]. Changsha:Hunan University, 2018.
[12]	Gopal G, Sankar H, Natarajan C, et al. Tetracycline removal using green synthesized bimetallic nZVI-Cu and bentonite supported green nZVI-Cu nanocomposite:A comparative study[J]. Journal of Environmental Management, 2020,254:109812.
[13]	陈苗,胡春华,郭昌胜,等.磁性Fe3O4纳米颗粒的制备及其催化降解水中磺胺甲恶唑研究[J].水资源与水工程学报, 2018,29(5):46-52. Chen M, Hu C H, Guo C S, et al. Synthesis of Fe3O4 magnetic nanoparticles and its application in catalytic degradation of sulfamethoxazole in water[J]. Journal of Water Resources and Water Engineering, 2018,29(5):46-52.
[14]	Huang R, Fang Z, Yan X, et al. Heterogeneous sono-Fenton catalytic degradation of bisphenol A by Fe3O4 magnetic nanoparticles under neutral condition[J]. Chemical Engineering Journal, 2012,197:242-249.
[15]	Xu J, Tan L, Baig S A, et al. Dechlorination of 2,4-dichlorophenol by nanoscale magnetic Pd/Fe particles:Effects of pH, temperature, common dissolved ions and humic acid[J]. Chemical Engineering Journal, 2013,231:26-35.
[16]	黄雪征,张永祥,田振军,等.纳米零价铁的制备、改性及场地应用研究进展[J].水处理技术, 2021,47(1):12-18,26. Huang X Z, Zhang Y X, Tian Z J, et al. Research progress in synthesis, modification and field application of nano zero-valent iron[J]. Technology of Water Treatment, 2021,47(1):12-18,26.
[17]	Tan L, Lu S, Fang Z, et al. Enhanced reductive debromination and subsequent oxidative ring-opening of decabromodiphenyl ether by integrated catalyst of nZVI supported on magnetic Fe3O4 nanoparticles[J]. Applied Catalysis B:Environmental, 2017,200:200-210.
[18]	刘焕联,李贤英,魏贝贝,等.超顺磁性纳米Fe3O4的制备及其类Fenton反应性能[J].环境工程学报, 2017,11(6):3525-3531. Liu H L, Li X Y, Wei B B, et al. Synthesis of super-paramagnetic Fe3O4 nanoparticles and its Fenton-like properties[J]. Chinese Journal of Environmental Engineering, 2017,11(6):3525-3531.
[19]	Lv X, Xu J, Jiang G, et al. Highly active nanoscale zero-valent iron (nZVI)-Fe3O4 nanocomposites for the removal of chromium (VI) from aqueous solutions[J]. Journal of Colloid and Interface Science, 2012, 369(1):460-469.
[20]	Fu F, Dionysiou D D, Liu H. The use of zero-valent iron for groundwater remediation and wastewater treatment:A review[J]. Journal of Hazardous Materials, 2014,267:194-205.
[21]	Sun X, Kurokawa T, Suzuki M, et al. Removal of cationic dye methylene blue by zero-valent iron:Effects of pH and dissolved oxygen on removal mechanisms[J]. Journal of Environmental Science and Health, Part A, 2015,50(10):1057-1071.
[22]	Kwan W P, Voelker B M. Rates of hydroxyl radical generation and organic compound oxidation in mineral-catalyzed Fenton-like systems[J]. Environmental Science&Technology, 2003,37(6):1150-1158.
[23]	Kitajima N, Fukuzumi S, Ono Y, et al. Formation of superoxide ion during the decomposition of hydrogen peroxide on supported metals[J]. The Journal of Physical Chemistry, 1978,82(13):1505-1509.
[24]	Wu H, Dou X, Deng D, et al. Decolourization of the azo dye Orange G in aqueous solution via a heterogeneous Fenton-like reaction catalysed by goethite[J]. Environmental Technology, 2012,33(14):1545-1552.
[25]	裴欢,毛飞,司友斌.纳米铁氧化物催化类Fenton反应降解抗生素磺胺[J].农业环境科学学报, 2015,34(7):1356-1362. Pei H, Mao F, Si Y B. Degradation of antibiotic sulfanilamide in aqueous solution via a heterogeneous fenton-like reaction catalyzed by nano-iron oxides[J]. Journal of Agro-Environment Science, 2015, 34(7):1356-1362.
[26]	邓景衡,文湘华,李佳喜.碳纳米管负载纳米四氧化三铁多相类芬顿降解亚甲基蓝[J].环境科学学报, 2014,34(6):1436-1442. Deng J H, Wen X H, Li J X. Degradation of methylene blue by heterogeneous Fenton-like reaction using Fe3O4/carbon nanotube composites[J]. Acta Scientiae Circumstantiae, 2014,34(6):1436-1442.
[27]	关英红,孙维敬,王盼盼.PMS/Fe0体系中自由基产率比及莠去津降解动力学[J].哈尔滨工业大学学报, 2022,54(2):50-58. Guan Y H, Sun W J, Wang P P. Radical production ratio and atrazine degradation kinetics in PMS/Fe0system[J]. Journal of Harbin Institute of Technology, 2022,54(2):50-58.
[28]	Wei X, Gao N, Li C, et al. Zero-valent iron (ZVI) activation of persulfate (PS) for oxidation of bentazon in water[J]. Chemical Engineering Journal, 2016,285:660-670.
[29]	林爱秋,程和发.芬顿及光芬顿法降解氟喹诺酮类抗生素研究进展[J].环境化学, 2021,40(5):1305-1318. Lin A Q, Cheng H F. Recent development in the degradation of fluoroquinolones by Fenton and photo-Fenton processes[J]. Environmental Chemistry, 2021,40(5):1305-1318.
[30]	Sun X, Qin Y, Zhou W. Degradation of amoxicillin from water by ultrasound-zero-valent iron activated sodium persulfate[J]. Separation and Purification Technology, 2021,275:119080.
[31]	Xekoukoulotakis N P, Drosou C, Brebou C, et al. Kinetics of UVA/TiO2 photocatalytic degradation and mineralization of the antibiotic sulfamethoxazole in aqueous matrices[J]. Catalysis Today, 2011, 161(1):163-168.
[32]	Kobayashi M, Kurosu S, Yamaguchi R, et al. Removal of antibiotic sulfamethoxazole by zero-valent iron under oxic and anoxic conditions:Removal mechanisms in acidic, neutral and alkaline solutions[J]. Journal of Environmental Management, 2017,200:88-96.
[33]	王磊,王海霞,吕效平.Fenton法处理水中4,4'-二溴联苯及动力学研究[J].环境科学与技术, 2007,(12):69-72,121. Wang L, Wang H X, Lv X P. Treatment of 4,4'-dibromobiphenyl aqueous solution by Fenton's reagent and its kinetics study[J]. Environmental Science&Technology, 2007,(12):69-72,121.
[34]	杨博.金属氧化物/石墨烯复合材料催化降解亚甲基蓝研究[D].兰州:兰州大学, 2015. Yang B. Study on the Degradation of methylene blue catalyzed by metal oxide/graphene composites[D]. Lanzhou:Lanzhou University, 2015.
[35]	白孟琦,李敏睿,丁欣欣,等.不同猝灭剂对SO4·-和·OH高级氧化体系的猝灭效果[J].工业水处理, 2021,41(8):75-80. Bai M Q, Li M R, Ding X X, et al. Quenching effect of different quenchers on SO4·- and ·OH based advanced oxidation processes[J]. Industrial Water Treatment, 2021,41(8):75-80.
[36]	Zhang X, Wang J, Duan B, et al. Degradation of sulfamethoxazole in water by a combined system of ultrasound/PW12/KI/H2O2[J]. Separation and Purification Technology, 2021,270:118790.
[37]	Huang Y, Yang J. Degradation of sulfamethoxazole by the heterogeneous Fenton-like reaction between gallic acid and ferrihydrite[J]. Ecotoxicology and Environmental Safety, 2021,226:112847.